Thin films of YBaCu(F)O were deposited on SrTiO3(100) substrates by multilayer deposition from three electron guns containing Y, BaF2, and Cu under a pressure of 5×10−5Torr of O2. The films were later annealed in a separate chamber under a flowing O2‐H2O atmosphere. X‐ray diffraction studies reveal that the resulting structure is highly oriented with theaaxis perpendicular to the substrate. Scanning electron micrographs show a morphology consisting of an array of orthogonal, interconnecting bars with well‐developed junctions. High‐resolution electron microscopy and electron diffraction patterns show that these junctions are atomically abrupt and that the associatedcaxes are mutually perpendicular. These epitaxial films show a sharp resistive transition withTc(R=0) as high as 90 K. The zero field critical current density, determined from magnetization measurements, is 2.9×106A/cm2at 4.2 K and 5.0×104A/cm2at 77 K.